Synergistic modulation of MOFs structure and carbon complex to enhance the integrated CO₂ adsorption and catalytic conversion

The integrated capture and catalytic conversion of CO₂ from industrial flue gas is a current research focus. Metal-organic frameworks （MOFs） are widely used in CO₂ adsorption and separation. To enhance the water stability of a copper-based MOF adsorbent-catalyst, a structure-directing agent （AspCuTEA） was employed to modulate its synthesis. This AspCuTEA was further integrated with hydrophobic carbon aerogel （CCA） to co-regulate the structure of a composite adsorbent-catalyst （AspCuTEA-CCA）, aiming to improve its performance for both CO₂ adsorption and conversion. In a cyclic fixed-bed system, the AspCuTEA-CCA was first used for CO₂ adsorption and separation. Subsequently, the adsorbed CO₂ was directly utilized for the cycloaddition reaction with epichlorohydrin to produce cyclic carbonate without a desorption step. Adsorption results showed that the AspCuTEA-CCA achieved saturated CO₂ capacities of 386 mg/g for pure CO₂ and 198 mg/g for a 15% CO₂ mixture. Notably, the presence of a small amount of water vapor enhanced CO₂ uptake. The direct catalytic conversion of the adsorbed CO₂ into cyclic carbonate reached a yield of 93.6%. The AspCuTEA-CCA maintained its structural integrity over 10 adsorption-desorption cycles and 3 catalytic conversion cycles, demonstrating excellent structural stability and consistent performance, indicating promising potential for industrial application.